Gradient High‐Q Dielectric Metasurfaces for Broadband Sensing and Control of Vibrational Light‐Matter Coupling

Abstract Surface‐enhanced infrared absorption spectroscopy (SEIRA) has emerged as a powerful technique for ultrasensitive chemical‐specific analysis. SEIRA can be realized by employing metasurfaces that can enhance light‐matter interactions in the spectral bands of molecular vibrations. Increasing sample complexity emphasizes the need for metasurfaces that can operate simultaneously at different spectral bands, both accessing rich spectral information over a broad band, and resolving subtle differences in the absorption fingerprints through narrow‐band resonances. Here, a novel concept of resonance‐gradient metasurfaces is introduced, where the required spectral selectivity is achieved via local high‐quality‐factor (high‐Q) resonances, while the continuous coverage of a broad band is enabled by the gradual adjustment of the unit‐cell dimensions along the planar structure. The highly tailorable design of the gradient metasurfaces provides flexibility for shaping the spectral sampling density to match the relevant bands of target analytes while keeping a compact device footprint. The versatility of the gradient metasurfaces is demonstrated through several sensing scenarios, including polymer mixture deconvolution, detecting a multistep bioassay, and identification of the onset of vibrational strong coupling regime. The proposed gradient‐resonance platform significantly contributes to the rapidly evolving landscape of nonlocal metasurfaces, enabling applications in molecular detection and analysis of fundamental light‐matter interaction phenomena.